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  • Letter

Distinguishing and controlling Mottness in 1T−TaS2 by ultrafast light

Changhua Bao1, Haoyuan Zhong1, Fei Wang1, Tianyun Lin1, Haoxiong Zhang1, Zhiyuan Sun1, Wenhui Duan1,2, and Shuyun Zhou1,2,*

  • 1State Key Laboratory of Low-Dimensional Quantum Physics and Department of Physics, Tsinghua University, Beijing 100084, People's Republic of China
  • 2Frontier Science Center for Quantum Information, Beijing 100084, People's Republic of China

  • *Author to whom correspondence should be addressed: syzhou@mail.tsinghua.edu.cn

Phys. Rev. B 107, L121103 – Published 15 March, 2023

DOI: https://doi.org/10.1103/PhysRevB.107.L121103

Abstract

Distinguishing and controlling the extent of Mottness is important for materials where the energy scales of the on-site Coulomb repulsion U and the bandwidth W are comparable. Here, we report the ultrafast electronic dynamics of 1T−TaS2 by ultrafast time- and angle-resolved photoemission spectroscopy. A comparison of the electron dynamics for the intermediate phase (I-phase) as well as the low-temperature commensurate charge density wave (C-CDW) phase shows distinctive dynamics. While the I-phase is characterized by an instantaneous response and nearly time-resolution-limited fast relaxation (∼200 fs), the C-CDW phase shows a delayed response and a slower relaxation (a few ps). Such distinctive dynamics reflect the different relaxation mechanisms and provide nonequilibrium signatures to distinguish the Mott insulating I-phase from the C-CDW band insulating phase. Moreover, a light-induced bandwidth reduction is observed in the C-CDW phase, pushing it toward the Mott insulating phase. Our work demonstrates the power of an ultrafast light-matter interaction in both distinguishing and controlling the extent of Mottness on the ultrafast timescale.

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